3D-interconnected hierarchical porous N-doped carbon supported ruthenium nanoparticles as an efficient catalyst for toluene and quinoline hydrogenation

摘要

Ruthenium nanoparticles (2.6 nm) uniformly dispersed on a three-dimensional (3D) interconnected hierarchical porous N-doped carbon (Ru/NHPC) have been successfully developed, serving as a highly active and stable catalyst for the selective hydrogenation of aromatics under mild conditions. A novel "leavening" strategy, i.e. using biomass-derived alpha-cellulose as a carbon precursor and ammonium oxalate as both a nitrogen source and foaming agent, affords the NHPC material a large surface area (870 m(2) g(-1)), an excellent hierarchical nanostructure which acts as a convenient mass transfer channel and a high ability in stabilizing and dispersing Ru nanoparticles. The Ru/NHPC catalyst exhibits a substantially enhanced activity for the hydrogenation of toluene (TOF up to 39 000 h(-1)) and quinoline (TOF up to 2858 h(-1)) in comparison with Ru/HPC (3D-hierarchical porous carbon without nitrogen doping) and Ru/AC (commercial activated carbon) under the same reaction conditions. Further investigations indicate that the 3D interconnected porous structure and N-doping contribute to the improved diffusion and mass transfer, homogeneous dispersion of ruthenium nanoparticles and high percentage of Ru-0 (active sites), which results in considerable catalytic performance. This work offers great potential for the application of supported catalysts based on NHPC materials in fine chemical production with high activity.